Enhanced Electrochemical CO₂ Reduction to Formate over Phosphate‐Modified In: Water Activation and Active Site Tuning

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 26, 2024

Electrochemical CO

Language: Английский

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Tailoring CO₂ Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) orientate the transition adsorption configuration from C,O-side O-end, which triggers a shift activated first-step protonation C–C coupling, thus switching target product HCOOH in Faraday efficiency (FE: 90.6%) on FeN2S2 CH3COOH 82.3%) Fe4S4/FeN2S2. The strength *OCHO upon solitary site is linearly related coordination number Fe–S, with predominantly produced over single-atom (ortho-substituted S atoms). Fe4S4 cluster functions as switch reduction product, can not only optimize electronic structure neighboring but also impel complete hydrocarbon intermediate *CH3, followed coupling CO2* *CH3 via synergistic catalysis This strategy provides new avenue modulate reactant model desirable pathways, potential applications diverse multistep electrochemical processes controlled selectivity.

Language: Английский

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Interfacial Electronic Interaction in Amorphous–Crystalline CeO_x‐Sn Heterostructures for Optimizing CO₂ to Formate Conversion

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 18, 2024

Abstract Formate, a crucial chemical raw material, holds significant promise for industrial applications in the context of CO 2 electroreduction reaction (CO RR). Despite its potential, challenges, such as poor selectivity and low formation rate at high current densities persist, primarily due to competing hydrogen evolution (HER) energy barriers associated with *OCHO intermediate generation. Herein, one‐step co‐reduction strategy is employed construct an amorphous–crystalline CeO x ‐Sn heterostructure, demonstrating remarkable catalytic performance converting formate. The optimized heterostructures reach density 265.1 mA cm −2 formate Faraday efficiency 95% −1.07 V versus RHE. Especially, achieves 444.4 production 9211.8 µmol h −1 −1.67 RHE, surpassing most previously reported materials. Experimental results, coupled （density functional theory）DFT calculations confirm that robust interface interaction between Sn active center induces electron transfer from crystalline site amorphous , some Ce 4+ get electrons convert unsaturated 3+ optimizing electronic structure Sn. This heterostructure promotes during RR, reducing barrier formed by intermediates, thus achieving efficient reduction

Language: Английский

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The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(41)

Published: July 12, 2024

The electrochemical CO

Language: Английский

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Enhanced Electrochemical CO2 Reduction to Formate over Phosphate‐Modified In: Water Activation and Active Site Tuning

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(27)

Published: April 26, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) offers a sustainable strategy for producing fuels and chemicals. However, it suffers from sluggish activation slow water dissociation. In this work, we construct (P−O) δ− modified catalyst that exhibits high activity selectivity in electrochemical to formate. A combination of situ characterizations kinetic analyses indicate has strong interaction with K + (H O) n , which effectively accelerates dissociation provide protons. attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) measurements together density functional theory (DFT) calculations disclose modification leads higher valence state active site, thus promoting HCOO* formation, while inhibiting competitive hydrogen evolution (HER). As result, the oxide‐derived excellent formate across broad potential window Faradaic efficiency as 92.1 % at partial current ~200 mA cm −2 cathodic −1.2 V vs. RHE an alkaline electrolyte.

Language: Английский

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Strategies for Improving Product Selectivity in Electrocatalytic Carbon Dioxide Reduction Using Copper‐Based Catalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(51)

Published: Aug. 29, 2024

Abstract As an effective approach to converting carbon oxide (CO 2 ) into value‐added carbonaceous products, the electrochemical CO reduction reaction (ECO RR) has shown considerable potential for neutrality, addressing global pollution and climate issues. Copper (Cu)‐based electrocatalysts (CuECs) are acknowledged as important candidates ECO RR of multi‐carbon products. Nevertheless, complicated electron transfer multiple competitive pathways in production process raise challenges product selectivity. While achieving high current density structural stability, improving selectivity CuECs become crucial their practical applications. Herein, overview fundamental thermodynamic kinetic principles presented. Then, typical strategies summarized increasing CuEC formation products from , including morphological control, component design, defect interface design. The catalyst catalytic performance, mechanisms involved these reviewed. Finally, major future prospects high‐performance discussed.

Language: Английский

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A Deep Insight into the Microscopic Dynamics of the Electrode–Electrolyte Interface under Extreme Operating Conditions

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 19, 2025

Understanding the interfacial dynamics during operation is critical for electrochemistry to make great advancements. However, breakthroughs on this topic under extreme conditions are very scarce. Here, as an example, we employ operando Raman spectroscopy decode of titanium electrolysis using a tailored instrument. Direct spectral evidence not only confirms two-step reduction pathway and key intermediate (TiF52-) in molten fluorides with high-temperature strong-corrosion but also unravels origins undesirable shuttling effect TiF52-, which sluggish kinetics outward diffusion behavior TiF52-. Moreover, insightful atomic scenario electric double layer (EDL) varied potentials has been established. These quantitative understandings guide us design economical-feasible regulation protocols─the rational combination high-concentration, low-valence Ti-ion electrolyte appropriate applied potential. Impressively, current efficiency greatly promoted from 27.7 81.8% our proposed protocols. Finally, work demonstrates bottom-up technological research paradigm based mechanism insights rather than phenomenological findings, will accelerate advancement electrochemistry.

Language: Английский

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Utilization of steelwork off-gases through methanol synthesis: Sulfur-induced dynamic migration of ZnOx over industrial Cu/ZnO/Al2O3 catalyst and the poisoning mechanism

Journal of Environmental Sciences, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 1, 2025

Language: Английский

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Cu-Thioamide coordination polymers derived Cu-S catalysts for CO2 electroreduction to formate

Fuel, Journal Year: 2025, Volume and Issue: 392, P. 134711 - 134711

Published: March 2, 2025

Language: Английский

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Enhanced electrocatalytic CO2 reduction through surface modification of Cu-based catalysts

Fuel, Journal Year: 2025, Volume and Issue: 392, P. 134576 - 134576

Published: March 5, 2025

Language: Английский

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